Regulating the Co Spin State via Directional Fe Doping to Enhance Sulfur Conversion Catalysis

Abstract In lithium‐sulfur (Li‐S) batteries, the sluggish redox kinetics of polysulfides and the severe shuttle effect remain major challenges. Herein, a Fe‐doped bimetallic heterostructure is rationally constructed on conductive carbon cloth (CC), which serves as a robust 3D scaffold with excellent electrical conductivity and low cost. The directionally doped Fe can regulate the spin state of the heterostructure, resulting in an upshift of energy levels and the generation of more active electronic states. This promotes stronger lithium polysulfides (LiPSs) adsorption, accelerates charge transfer, and enhances redox kinetics. Consequently, this novel S host delivers a 1075.5 mAh g −1 capacity at 0.2 C after 100 cycles and an ultralow capacity decay of 0.022% per cycles at 1 C over 500 cycles, showcasing excellent cycling stability. This work offers a promising strategy for developing efficient electrocatalysts for Keywords